期刊
APPLIED CATALYSIS B-ENVIRONMENTAL
卷 270, 期 -, 页码 -出版社
ELSEVIER
DOI: 10.1016/j.apcatb.2020.118888
关键词
CH4 electrooxidation; C-H activation; C-C coupling; Ethanol; NiO/Ni interface
资金
- National Natural Science Foundation of China [91745114, 21802160, 21473233]
- Ministry of Science and Technology of China [2016YFA0202800, 2018YFB0604700]
- Shanghai Sailing Program [18YF1425700]
- Shanghai Functional Platform for Innovation Low Carbon Technology
- Hundred Talents Program of Chinese Academy of Sciences
Electrocatalytic conversion of methane (CH4) to valuable chemicals under mild conditions is an attractive approach that combines the direct utilization of natural gas as a hydrocarbon feedstock and the chemical storage of renewable electricity. However, it remains a great challenge due to the intrinsic chemical inertness of CH4. Here we report that a NiO/Ni interface constructed by calcination can act as the active site for the electrooxidation of CH4 to alcohols especially ethanol. With the optimized NiO/Ni interface catalyst, an 89 % Faradaic efficiency (FE) for ethanol production with a yield of 25 mu mol.g(NiO)(-1).h(-1) at 1.40 V versus reversible hydrogen electrode (RHE) was achieved. Experiments and density functional theory (DFT) calculations demonstrated that the NiO/Ni interface enables efficient C-H activation and C-C coupling, leading to the highly selective formation of ethanol from CH4 electrooxidation.
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